Operando-informed precatalyst programming towards reliable high-current-density electrolysis

Lu Xia; Bruna Ferreira Gomes; Wulyu Jiang; Daniel Escalera-López; Yang Wang; Yang Hu; Alaa Y Faid; Kaiwen Wang; Tengyu Chen; Kaiqi Zhao; Xu Zhang; Yingtang Zhou; Ranit Ram; Barbara Polesso; Anku Guha; Jiaqi Su; Carlos M S Lobo; Michael Haumann; Robert Spatschek; Svein Sunde; Lin Gan; Ming Huang; Xiaoyuan Zhou; Christina Roth; Werner Lehnert; Serhiy Cherevko; Liyong Gan; F Pelayo García de Arquer; Meital Shviro

doi:10.1038/s41563-025-02128-7

Operando-informed precatalyst programming towards reliable high-current-density electrolysis

Nat Mater. 2025 May;24(5):753-761. doi: 10.1038/s41563-025-02128-7. Epub 2025 Feb 28.

Authors

Lu Xia^#^{1

2}, Bruna Ferreira Gomes^#³, Wulyu Jiang^#¹, Daniel Escalera-López⁴, Yang Wang⁵, Yang Hu⁶, Alaa Y Faid⁷, Kaiwen Wang², Tengyu Chen², Kaiqi Zhao², Xu Zhang⁸, Yingtang Zhou⁹, Ranit Ram², Barbara Polesso², Anku Guha², Jiaqi Su¹⁰, Carlos M S Lobo³, Michael Haumann¹¹, Robert Spatschek⁶, Svein Sunde⁷, Lin Gan¹², Ming Huang¹³, Xiaoyuan Zhou⁵, Christina Roth³, Werner Lehnert^{1

14}, Serhiy Cherevko⁴, Liyong Gan¹⁵, F Pelayo García de Arquer¹⁶, Meital Shviro^{17

18}

Affiliations

¹ Institute of Energy Technologies, Electrochemical Process Engineering, Forschungszentrum Jülich, Jülich, Germany.
² Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology, Castelldefels, Spain.
³ Electrochemical Process Engineering, University of Bayreuth, Bayreuth, Germany.
⁴ Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy, Forschungszentrum Jülich, Erlangen, Germany.
⁵ College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing, P. R. China.
⁶ Institute of Energy Materials and Devices, Microstructure and Properties of Materials, Forschungszentrum Jülich, Jülich, Germany.
⁷ Department of Materials Science and Engineering, Norwegian University of Science and Technology, Trondheim, Norway.
⁸ Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, China.
⁹ National Engineering Research Center for Marine Aquaculture, Marine Science and Technology College, Zhejiang Ocean University, Zhoushan, China.
¹⁰ Department of Health Sciences and Technology, ETH Zurich, Zurich, Switzerland.
¹¹ Department of Physics, Freie Universität Berlin, Berlin, Germany.
¹² Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China.
¹³ Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, China.
¹⁴ Faculty of Mechanical Engineering, RWTH Aachen University, Aachen, Germany.
¹⁵ College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing, P. R. China. ganly@cqu.edu.cn.
¹⁶ Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology, Castelldefels, Spain. pelayo.garciadearquer@icfo.eu.
¹⁷ Institute of Energy Technologies, Electrochemical Process Engineering, Forschungszentrum Jülich, Jülich, Germany. meital.shviro@nrel.gov.
¹⁸ Chemistry and Nanoscience Center, National Renewable Energy Laboratory, Golden, CO, USA. meital.shviro@nrel.gov.

^# Contributed equally.

PMID: 40021826
DOI: 10.1038/s41563-025-02128-7

Abstract

Electrocatalysts support crucial industrial processes and emerging decarbonization technologies, but their design is hindered by structural and compositional changes during operation, especially at application-relevant current densities. Here we use operando X-ray spectroscopy and modelling to track, and eventually direct, the reconstruction of iron sulfides and oxides for the oxygen evolution reaction. We show that inappropriate activation protocols lead to uncontrollable Fe oxidation and irreversible catalyst degradation, compromising stability and reliability and precluding predictive design. Based on these, we develop activation programming strategies that, considering the thermodynamics and kinetics of surface reconstruction, offer control over precatalyst oxidation. This enables reliable predictions and the design of active and stable electrocatalysts. In a Ni_xFe_1-xS₂ model system, this leads to a threefold improvement in durability after programmed activation, with a cell degradation rate of 0.12 mV h^-¹ over 550 h (standard operation: 0.29 mV h^-¹, constrained to 200 h), in an anion exchange membrane water electrolyser operating at 1 A cm^-². This work bridges predictive modelling and experimental design, improving the electrocatalyst reliability for industrial water electrolysis and beyond at high current densities.

Abstract

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